TY - JOUR

T1 - Methane conversion to syngas and hydrogen in a dual phase Ce0.8Sm0.2O2-Δ-Sr2Fe1.5Mo0.5O5+Δ membrane reactor with improved stability

AU - Liang, Wenyuan

AU - Zhou, Hangyue

AU - Caro, Jürgen

AU - Jiang, Heqing

N1 - Funding Information: This work was financially supported by National Natural Science Foundation of China (No. 21471156 , 21501186 ), the State Key Laboratory of Coal Conversion (No: J15-16-907 ), the China Postdoctoral Science Foundation ( 2018M632739 ), the Natural Science Foundation of Shandong Province ( ZR2017BB082 ). Mr. W. Liang thanks financial support from the China Scholarship Council (CSC) .

PY - 2018/8/2

Y1 - 2018/8/2

N2 - Coupling of partial oxidation of methane (POM) with water dissociation in an oxygen transport membrane is a promising technology for methane utilization. However, cobalt-based membrane materials show poor stability under the above harsh conditions. In this work, a nominal 60 wt % Ce0.8Sm0.2O2-δ-40 wt % Sr2Fe1.5Mo0.5O5+δ (CSO-SFMO) dual phase membrane is reported, which was synthesized by using a one-pot EDTA-citric acid complexing method. The phase structure and morphology of the CSO-SFMO membrane were characterized by XRD, SEM and EDXS. It was found that a uniform distribution of CSO phase with a fluorite structure and SFMO phase with a perovskite structure was achieved in the dual phase membrane. The CSO-SFMO membrane exhibited an improved stability compared with cobalt based perovskite Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) membrane under CO2 or reductive gas atmospheres. The oxygen permeation flux of the dual phase membrane was investigated under different oxygen partial pressure gradients: air/He, air/CO2, air/POM, and H2O/POM. At 950 °C, the oxygen permeation fluxes of the CSO-SFMO membrane under air/POM and H2O/POM gradients were 2.7 cm3 (STP) min−1 cm−2 and 0.75 cm3 (STP) min−1 cm−2, respectively, which were much higher than the oxygen flux of 0.1 cm3 (STP) min−1 cm−2 under air/He. Moreover, a CO selectivity of 98%, a CH4 conversion of 97% on the POM side and a H2 production of 1.5 cm3 (STP) min−1 cm−2 on the H2O splitting side were achieved in CSO-SFMO membrane reactor under the oxygen partial pressure gradient of H2O/POM, which was steadily run for 100 h before the measurement was intentionally stopped.

AB - Coupling of partial oxidation of methane (POM) with water dissociation in an oxygen transport membrane is a promising technology for methane utilization. However, cobalt-based membrane materials show poor stability under the above harsh conditions. In this work, a nominal 60 wt % Ce0.8Sm0.2O2-δ-40 wt % Sr2Fe1.5Mo0.5O5+δ (CSO-SFMO) dual phase membrane is reported, which was synthesized by using a one-pot EDTA-citric acid complexing method. The phase structure and morphology of the CSO-SFMO membrane were characterized by XRD, SEM and EDXS. It was found that a uniform distribution of CSO phase with a fluorite structure and SFMO phase with a perovskite structure was achieved in the dual phase membrane. The CSO-SFMO membrane exhibited an improved stability compared with cobalt based perovskite Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) membrane under CO2 or reductive gas atmospheres. The oxygen permeation flux of the dual phase membrane was investigated under different oxygen partial pressure gradients: air/He, air/CO2, air/POM, and H2O/POM. At 950 °C, the oxygen permeation fluxes of the CSO-SFMO membrane under air/POM and H2O/POM gradients were 2.7 cm3 (STP) min−1 cm−2 and 0.75 cm3 (STP) min−1 cm−2, respectively, which were much higher than the oxygen flux of 0.1 cm3 (STP) min−1 cm−2 under air/He. Moreover, a CO selectivity of 98%, a CH4 conversion of 97% on the POM side and a H2 production of 1.5 cm3 (STP) min−1 cm−2 on the H2O splitting side were achieved in CSO-SFMO membrane reactor under the oxygen partial pressure gradient of H2O/POM, which was steadily run for 100 h before the measurement was intentionally stopped.

KW - Hydrogen

KW - Oxygen transport membrane

KW - Partial oxidation of methane (POM)

KW - Water splitting

UR - http://www.scopus.com/inward/record.url?scp=85049003363&partnerID=8YFLogxK

U2 - 10.1016/j.ijhydene.2018.06.008

DO - 10.1016/j.ijhydene.2018.06.008

M3 - Article

AN - SCOPUS:85049003363

VL - 43

SP - 14478

EP - 14485

JO - International Journal of Hydrogen Energy

JF - International Journal of Hydrogen Energy

SN - 0360-3199

IS - 31

ER -